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Room-Temperature Micron-Scale Exciton Migration in a Stabilized Emissive Molecular Aggregate.

  • Author(s): Caram, Justin R;
  • Doria, Sandra;
  • Eisele, Dörthe M;
  • Freyria, Francesca S;
  • Sinclair, Timothy S;
  • Rebentrost, Patrick;
  • Lloyd, Seth;
  • Bawendi, Moungi G
  • et al.
Abstract

We report 1.6 ± 1 μm exciton transport in self-assembled supramolecular light-harvesting nanotubes (LHNs) assembled from amphiphillic cyanine dyes. We stabilize LHNs in a sucrose glass matrix, greatly reducing light and oxidative damage and allowing the observation of exciton-exciton annihilation signatures under weak excitation flux. Fitting to a one-dimensional diffusion model, we find an average exciton diffusion constant of 55 ± 20 cm2/s, among the highest measured for an organic system. We develop a simple model that uses cryogenic measurements of static and dynamic energetic disorder to estimate a diffusion constant of 32 cm2/s, in agreement with experiment. We ascribe large exciton diffusion lengths to low static and dynamic energetic disorder in LHNs. We argue that matrix-stabilized LHNS represent an excellent model system to study coherent excitonic transport.

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